Chin. Sci. Bull. (2014) 59(23):2882–2889
com
DOI 10.1007/s11434-014-0388-1
Article
Mineralization of flue gas CO2 with coproduction of valuable
magnesium carbonate by means of magnesium chloride
Heping Xie • Yufei Wang • Wei Chu •
Yang Ju
Received: 3 February 2014 / Accepted: 9 April 2014 / Published online: 14 May 2014
Ó Science China Press and Springer-Verlag Berlin Heidelberg 2014
Abstract CO2 mineralization and utilization is a new
area for reducing the CO2 emissions. By reacting with
natural mineral or industrial waste, CO2 can be transformed
into valuable solid carbonate (such as calcium carbonate or
magnesium carbonate) with recovery of some products
simultaneously. In this paper, a novel method was proposed
to mineralize CO2 by means of magnesium chloride with
small energy consumption. In this method, magnesium
chloride was firstly transformed into magnesium hydroxide
by electrolysis. The formed magnesium hydroxide showed
high reactivity to mineralize CO2. In our study, even at low
concentration, CO2 can be effectively mineralized by this
method, which makes it possible to directly mineralize flue
gas CO2, avoiding the expensive process of CO2 capture
and purification. Moreover, valuable products such as
hydromagnesite and nesquehonite can be recovered by this
method. Because of the wide distribution of magnesium
chloride in nature, large-scale CO2 mineralization is
potential by means of magnesium chloride.
H. Xie (&)  Y. Wang  W. Chu
Center of CCUS and CO2 Mineralization and Utilization,
Sichuan University, Chengdu 610065, China
e-mail: xiehp@scu.edu.cn
H. Xie  Y. Wang
Key Laboratory of Energy Engineering Safety and Mechanics on
Disasters, The Ministry of Education, Sichuan University,
Chengdu 610065, China
W. Chu
School of Chemical Engineering, Sichuan University,
Chengdu 610065, China
Y. Ju
State Key Laboratory of Coal Resources and Safe Mining, China
University of Mining Technology, Beijing 100083, China
123
csb.scichina.
www.springer.com/scp
Environmental Science & Technology
Keywords CO2 mineralization and utilization 
CCUS  Magnesium chloride  Electrolysis 
Magnesium carbonate
1 Introduction
The emission of CO2 by combustion of fossil fuel is con-
sidered the main cause of global warming and a great threat
to human environment. Reducing the emissions of CO2
becomes a worldwide event [1–5]. Currently, Carbon
dioxide Capture and Storage (CCS) is considered the most
potential method for reducing the emission of CO2. In the
process of CCS, industrial flue gas CO2, the concentration
of which is usually 10 %–20 %, is firstly captured and
purified. And then the pure CO2 was sequestrated by
methods of geological storage, ocean storage or mineral
carbonation.
Currently, chemical absorption is the main method for
CO2 capture and the energy consumption for capturing per
metric ton of pure CO2 from industrial fuel gas is
370–510 kWh. Among the methods of CO2 storage, CO2
geological storage has been heatedly studied. There are
pilot-scale and full-scale CO2 sequestration sites currently
operating around the world, such as those in Texas, USA
and Erdos, China [6–10]. However, because of the high cost
and uncertain safety problem, the wide application of CO2
geological storage was constrained at the present stage.
CO2 mineralization and utilization is a new area for
disposal of CO2. The basic concept of CO2 mineralization
and utilization is using natural mineral or industrial by-
products to react with CO2 and transform it into valuable
solid carbonate (such as calcium carbonate and magne-
sium carbonate), with coproduction of useful products
[11–13].
Chin. Sci. Bull. (2014) 59(23):2882–2889
Nowadays, the raw materials for CO2 mineralization are
focused on olivine, serpentine and other natural alkaline
silicate [14–18]. The reaction between CO2 and silicate
minerals can be naturally occurred in nature, but this pro-
cess is too slow to be used for large-scale CO2 reduction in
short time. A number of works have been attempted to
accelerate the rate of CO2 mineralization [19–21]. Miner-
alization of CO2 in high temperature and high partial
pressure of CO2 with small particle size of silicates showed
faster reaction rate, but the high energy cost made it hard to
be industrially used [22]. Moreover, mixture of silica and
carbonates were obtained by these methods, but the
application of these products was limited.
Industrial by-products are other raw materials for CO2
mineralization [23–26]. In comparison, industrial by-pro-
ducts tend to be more reactive than natural silicate min-
erals. Cement kiln dust, coal fly ash, municipal solid waste
and steel-making slag are main industrial by-products used
for CO2 mineral carbonation. Although the industrial by-
products show an attractive reactivity, the total amount of
CO2 to be potentially sequestrated by industrial by-pro-
ducts, is limited because of the relatively small production
amount of industrial by-products.
Magnesium chloride is an earth-abundant resource,
which is widely distributed in sea water, salt lake, and
mine. The average concentration of magnesium ion in sea
water is about 0.13 %. The total number of CO2 emission
in 2010 was 30.06 billion tons [27]. If 0.1 % of the mag-
nesium chloride in the sea water was used for CO2 min-
eralization and CO2 was mineralized as magnesium
carbonate, 3.34 tribillion tons of CO2 could be mineralized
in theoretical value. It means that 0.1 % of the magnesium
chloride in sea water can potentially mineralize as much as
111 years’ amount of global CO2 emissions. There are
abundant magnesium salts in China. The concentration of
magnesium ion in surrounding sea water is 0.13 % and the
prospective reserves of magnesium salt in 4 major saline
lakes are as high as several billion tons. Moreover, 33 brine
lakes existed in Qaidam Basin, reserving most abundant
magnesium resources in China. A possible reaction
between CO2 and magnesium chloride is given in Eq. (1).
Hydromagnesite could be produced if this reaction occur-
red. Hydromagnesite is wildly used as resistant fireproof
insulation materials, and also used as raw materials for
manufacture of high-grade glass products, such as pig-
ment, paint and chemicals. Because of the wide applica-
tion of product and the wide distribution of raw material,
large-scale CO2 is potential to be mineralized by means of
magnesium chloride.
5MgCl2 þ 4CO2 þ 10H2 O ! Mg5 ðCO3 Þ4 ðOHÞ2 4H2 O
þ 10HCl
ð1Þ
2883
However, there are few reports on CO2 mineralization via
reaction with solution of magnesium chloride so far.
Therefore, how to mineralize CO2 with magnesium chloride
with recovery of valuable magnesium carbonate is the main
goal of our study. Moreover, because of the high energy
consumption of CO2 capture and purification, the other aim of
our work is finding a feasible way to directly mineralize flue
gas CO2, avoiding the process of CO2 capture.
In this paper, a novel method was proposed to miner-
alize flue gas CO2 by means of magnesium chloride. This
method aims at mineralizing CO2 and recovering valuable
magnesium carbonate with small energy consumption. In
this method, magnesium chloride was transformed into
magnesium hydroxide with recovery of hydrochloric acid
by electrolysis. Then the formed magnesium hydroxide
was reacted with acidic CO2, transforming CO2 into
magnesium bicarbonate solution. Finally, the magnesium
bicarbonate was decomposed into valuable magnesium
carbonate. The whole process can be shown as Fig. 1.
The electrolysis cell, used for transforming magnesium
chloride into magnesium hydroxide is shown in Fig. 2. The
electrolysis cell was divided into two compartments by
anion exchange membrane. Hydrogen gas diffusion elec-
trode was used as the anode to transforming H2 into H?.
Hydrogen gas diffusion electrode was firstly derived from
fuel cell, and it consisted of current collecting layer, cat-
alyst layer and carbon paper [28–30]. Nickel foil was used
as cathode in this work. During electrolysis, water was
electrolyzed and transformed into hydrogen and hydroxyl
ions at the cathode. The magnesium ions in solution were
precipitated into magnesium hydroxide via combining with
hydroxyl ions in solution. Because only anion was allowed
to pass through the anion exchange membrane, the mixture
of Mg(OH)2 and H? was avoided.
Cathode: 2H2 O þ Mg2þ þ 2e ! MgðOHÞ2 þ H2
ð2Þ
Anode: H2 ! 2Hþ þ 2e ð3Þ
This paper studied the feasibility of CO2 mineralization
by means of magnesium chloride with coproduction of
valuable magnesium carbonates. Moreover, the possibility
of directly mineralizing flue gas CO2 by the method was
Fig. 1 Process of CO2 mineralization by means of magnesium
chloride
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Fig. 2 Illustration of electrolysis cell for conversion of magnesium
chloride into magnesium hydroxide
also studied. The key factors, which influenced the
mineralizing process, such as cell voltage, the
concentration of hydrochloric acid, CO2 partial pressure
and decomposition temperature were also investigated.
2 Materials and methods
2.1 Materials
The magnesium chloride, sodium chloride and hydrochlo-
ric acid used in the experiment were of analytical grade.
The CO2, N2 and H2 were purchased from Dong Feng
Company (China) with the purity of 99.99 %. Hydrogen
gas diffusion electrodes, covered 1 mg/cm2 of platinum/C
as the catalyst, were bought from Shanghai Hesen Elec-
trical Co., Ltd. Anion exchange membrane was bought
from China Iontech Company.
2.2 Experimental process
2.2.1 Electrolysis of magnesium chloride solution
Hydrochloric acid with different concentration (0–1.6 mol/L)
was used as anolyte and the solution of magnesium chlo-
ride (1 mol/L) was used as catholyte. The electrolysis was
taken place with a setting current density. The concentra-
tion change of hydrochloric acid in anolyte compartment
was measured by acid-base titration. After reaction, the
product in catholyte compartment was filtrated, washed and
dried at 110 °C. The solid obtained was magnesium
hydroxide.
The change of current density with cell voltage was
tested and recorded when different concentration of
hydrochloric acid was added in anolyte compartment. In
most cases, magnesium chloride was coexisted with
sodium chloride in nature. So the solutions of sodium
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Chin. Sci. Bull. (2014) 59(23):2882–2889
chloride and magnesium chloride with different concen-
tration were used as catholyte and the change of current
density with cell voltage were tested.
2.2.2 Mineralization of CO2 at different concentration
The magnesium hydroxide, obtained by electrolysis, was
putted into a 250 mL three-necked flask and 100 mL water
was added in with agitation. The flue gas CO2 was imitated
by mixture of CO2 and N2. The mixed gas was bubbled into
the flask and reacted with magnesium hydroxide. The
mineralization reaction was conducted at room temperature
and the stirring speed was 350 r/min. The concentration of
CO2 was controlled at 20 %–100 % by adjusting the flow
rate of N2 and CO2, 1 mL solution in flask was removed
out every 15–30 min with needle syringe during the reac-
tion. After filtration, the concentration of bicarbonate in
solution was tested by acid-base titration. When the con-
centration of bicarbonate in solution stayed constant, the
reaction was stopped.
2.2.3 Formation of magnesium carbonate
The solution of magnesium bicarbonate was added into a
250 mL beaker and heated in a water bath at different
temperatures (25 °C, 80 °C) Then the solution of magne-
sium bicarbonate was stirred until a large number of solid
was precipitated. Finally, the solid was filtered, washed and
oven-dried at 60 °C.
2.3 Characterization and analysis of mineralization
products
The crystal properties of solid products, obtained during
the experiment, were determined by XRD. The sam-
ple morphology was studied by scanning electron micros-
copy (SEM). The thermal stability of the products in the
air was analyzed by Thermogravimetric Analysis (TGA).
TGA experiments were performed to characterize the
decomposition behavior of magnesium carbonate product.
The air was utilized as the carrier gas, with a heating rate of
20 °C/min in the temperature range of 25–800 °C. The
sample loading was typically 20 mg.
3 Results and discussion
3.1 Current efficiency of electrolysis
The current efficiency was represented by the ratio of the
amount of products actually produced to that theoretically
calculated by Faraday’s law of electrolysis. During elec-
trolysis, the concentration of hydrochloric acid in anolyte
Chin. Sci. Bull. (2014) 59(23):2882–2889
Fig. 3 Dependence of current efficiency with concentration of proton
in anolyte compartment
compartment was increasing. Figure 3 shows the depen-
dence of current efficiency with concentration of proton in
anolyte compartment. In our study, the current efficiency of
CO2 mineral carbonation reached about 98 % when con-
centration of acid was low (about 0.1 mol/L), but the
current efficiency decreased gradually with the concentra-
tion increasing of acid. When the concentration of hydro-
chloric acid was 1.6 mol/L, the current efficiency reduced
to 63 %. The observations can be explained as that a part of
proton in anolyte compartment passes through the AEM
and goes into catholyte compartment when the acid con-
centration is high. This phenomenon is called proton
leakage. In order to enhance the current efficiency of CO2
mineral carbonation at high concentration of acid, the
AEM should be revised to avoid proton leakage.
The leakage of proton can be avoided by improving the
selectivity of anion exchange membrane. In Ref. [29],
ARA membrane from Solvay shows a high selectivity. The
current efficiency could be still above 75 % when the
proton concentration reached 4.5 mol/L. So the perfor-
mance of anion exchange membrane has great influence on
the current efficiency. Improving the selectivity of anion
exchange membrane is one of the further directions of
study.
3.2 The reactivity of magnesium hydroxide for CO2
mineralization
According to Jung’s study [31], CO2 can be absorbed by
magnesium hydroxide in water (Eq. (4)) with relatively
fast reaction rate. In our study, formed magnesium
hydroxide was used to mineralize different concentration
CO2 (20 %, 50 %, 70 % and 100 %). The change of
bicarbonate concentration in solution is shown in Fig. 4. It
can be shown that CO2 with concentration of 20 % can be
2885
Fig. 4 Change of the concentration of bicarbonate with reaction time
on stream
directly reacted with magnesium hydroxide and trans-
formed into magnesium bicarbonate. Thus, it is feasible to
directly mineralize low concentration of CO2 by this
method. But the higher the CO2 concentration was, the
faster the mineralization rate became and the higher the
equilibrium concentration of magnesium bicarbonate
reached. When pure CO2 was used as raw material, the
concentration of bicarbonate in solution stayed at 0.4 mol/L
after 100 min. But, the concentration of bicarbonate was
0.2 mol/L after 400 min when the initial concentration of
CO2 was set at 20 %.
This study confirmed that the magnesium hydroxide was
reactive to directly mineralize low concentration of CO2.
Moreover, the slurry of magnesium hydroxide was also
used for Flue Gas Desulfurization (FGD) [32]. After FDG,
SO2 was transformed to soluble magnesium sulfate, so the
process of FGD wouldn’t influence the purity of magne-
sium carbonates formed by CO2 mineralization.
2CO2 þ MgðOHÞ2 ! MgðHCO3 Þ2 ð4Þ
It can be shown in Fig. 4, during the reaction of
magnesium hydroxide and CO2, the concentration of
bicarbonate was slightly increased at the beginning of the
reaction, but decreased afterward and then it significantly
increased and stayed in certain value finally. The reason
for this phenomenon was that the solubility of
solid magnesium hydroxide in water was low, and it is in
the form of solid in water. When the concentration of
bicarbonate reached a certain value, the bicarbonate would
react with magnesium ion on the surface of magnesium
hydroxide, and magnesium carbonate was formed. Thus,
the concentration of bicarbonate in solution would be
decreased in the second period. XRD results proved that
there was the formation of MgCO33H2O when the reaction
time on stream was about 30 min, while the concentration
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Fig. 5 Results of XRD analysis before reaction and after 30 min’s
reaction
of magnesium bicarbonates was slightly decreasing (shown
in Fig. 5). Both of magnesium carbonate and magnesium
hydroxide can react with CO2 and magnesium bicarbonate
was produced, so the concentration of magnesium
bicarbonate was increased again at the third period, until
the concentration of magnesium bicarbonate in solution
was saturated.
3.3 Mineral composition and thermal stability of solid
products
Different kinds of magnesium carbonate mineral can be
obtained when the solution of magnesium bicarbonate
decomposed at different temperature. Figure 6 shows the
XRD results of products. When the decomposing temperature
was 25 °C, the product was nesquehonite (MgCO33H2O).
When the temperature of decomposition was 80 °C, the
product was hydromagnesite (Mg5(CO3)4(OH)24H2O). The
SEM images of solid products showed that the surface mor-
phology of nesquehonite was in shape of elongated rectan-
gular (shown in Fig. 7a), and the hydromagnesite showed the
structure of petal (shown in Fig. 7b).
The TGA results showed that the nesquehonite had two
significant weight loss stages in the temperature range of
100–300 °C and 300–550 °C (shown in Fig. 8). This result
was consistent with that of Rao’s study [33]. The weigh
loss of MgCO33H2O in the range of 100–330 °C is due to
the loss of crystal water. In the range of 350–550 °C,
MgCO3 was decomposed into CO2 and MgO. Therefore,
the decomposition product of magnesium bicarbonate at
room temperature was nequeshonite, and the MgCO33H2O
had good thermal stability in the air.
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Chin. Sci. Bull. (2014) 59(23):2882–2889
Fig. 6 XRD results of obtained products
As shown in Fig. 8, the decomposition product for
magnesium bicarbonate solution obtained at 80 °C had
three weight loss stages in the temperature range of
200–280 °C, 400–500 °C and 500–560 °C, which was
consistent with TGA curve of hydromagnesium. The first
two stages of weight loss were due to the loss of crystal
water and water molecules in hydroxide, and the weight
loss at higher than 500 °C was due to the release of CO2
[34]. It proved that hydromagnesite also had good thermal
stability in the air, and CO2 can be safely sequestrated as
hydromagensite.
3.4 Cell voltage and energy consumption
of electrolysis
Figure 9 shows the plots of current density with cell volt-
age when different concentration of hydrochloric acid was
used as anolyte. The current started to be formed and redox
reaction occurred at the voltage of 0.60–0.62 V. With the
increase of HCl concentration in anolyte compartment, the
change of current density with cell voltage became more
dramatically. It was due to that the ionic strength of anolyte
was enhanced when concentration of hydrochloric acid
increased. Figure 10 shows the plots of current density
with cell voltage when mixed solutions of different con-
centration of sodium chloride and magnesium chloride
were used as catholyte. It showed that when the concen-
tration of chloride ion in solution was unchanged, the
change of concentration of sodium chloride and
Chin. Sci. Bull. (2014) 59(23):2882–2889
Fig. 7 Surface morphologies of obtained products. a Decomposition product of magnesium bicarbonate at room temperature, 25 °C;
b Decomposition product of magnesium bicarbonate at 80 °C
Fig. 8 TGA results of the products obtained at different decompo-
sition temperatures
magnesium chloride had nearly no influence on the change
of current density with cell voltage.
The main energy consumption for CO2 mineralization
by means of magnesium chloride was the energy consumed
for electrolysis. The energy consumption of electrolysis
was related to cell voltage and current efficiency.
Based on the theoretical value, the minimum cell volt-
age required for electrolysis of magnesium chloride was
only 0.38 V, and 473 kWh was required for mineralizing
per ton of CO2. In our study, the electrolysis of magnesium
chloride was occurred at the voltage of 0.60–0.62 V. At
this voltage, the electrolysis of magnesium chloride was
occurred, but reaction rate was too slow. The reaction rate
could be increased by improving the cell voltage, results in
increasing of energy consumption. When the cell voltage
was 0.7 V and 0.1 mol/L HCl was used as anolyte, the
energy required for mineralizing per ton of CO2,
2887
Fig. 9 Plots of current density versus cell voltage when different
concentration of hydrochloric acid was used as anolyte
coproduction of 3.16 tons of nesquehonite was about 871
kWh. Assuming the electric price to be 0.5 RMB/kWh, the
main cost for mineralizing per tons of CO2 was 435.5
RMB. Because the market price of main product,
nesquehonite, was about 3,000 RMB/t and 3.16 tons of
nesquehonite could be obtained when per ton of CO2 was
mineralized, the value of product reached as much as 9,480
RMB. Therefore, CO2 mineralization by means of mag-
nesium chloride was potentially to be industrial used.
4 Conclusions
Magnesium chloride is a kind of compound which is
widely distributed and abundant on earth. This research
reports a new alternative method for mineralizing flue gas
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Fig. 10 Plots of current density versus cell voltage when different
concentration of sodium chloride and magnesium chloride was used
as catholyte
carbon dioxide by means of magnesium chloride. In this
method, magnesium chloride was firstly transformed into
magnesium hydroxide by electrolysis. The formed mag-
nesium hydroxide showed high reactivity to mineralize
CO2 and the solution of magnesium bicarbonate was gen-
erated. Finally, the solution of magnesium bicarbonate was
decomposed, and valuable nesquehonite or hydromagne-
sium was generated.
By this method, CO2 at 20 % concentration can be
directly mineralized. It shows that it is possible to miner-
alize industrial flue gas CO2 directly, avoiding the high
energy-consuming process of CO2 capture and purification.
The main energy consumption for CO2 mineralization
by means of magnesium chloride was the energy consumed
for electrolysis. In our study, the electrolysis of magnesium
chloride was occurred at the voltage of 0.60–0.62 V, and
the reaction rate could be increased by improving the cell
voltage. When the cell voltage was 0.7 V and 0.1 mol/L
HCl was used as anolyte, the energy required for miner-
alizing per ton of CO2 with production of 3.16 tons of
nesquehonite was about 871 kWh (about 435.5 RMB).
At present, the market price of nesquehonite is about
3,000 RMB. Therefore, CO2 mineralization by means of
magnesium chloride is an efficient and economical way to
reduce the emissions of CO2, providing an alternative for
disposal of CO2.
Acknowledgments This work was supported by International
Cooperative Research Project of the Ministry of Science and Tech-
nology (2012DFA60760), the Natural Science Foundation of China
(51120145001, 51254002), the National Natural Science Funds for
Distinguished Young Scholars (51125017), and the Natural Basic
Research Projects of China (2011CB201201, 2010CB226804).
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Chin. Sci. Bull. (2014) 59(23):2882–2889
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